CN1347562A - Rechargeable hybrid battery/surpercapacitor system - Google Patents
Rechargeable hybrid battery/surpercapacitor system Download PDFInfo
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- CN1347562A CN1347562A CN00806515A CN00806515A CN1347562A CN 1347562 A CN1347562 A CN 1347562A CN 00806515 A CN00806515 A CN 00806515A CN 00806515 A CN00806515 A CN 00806515A CN 1347562 A CN1347562 A CN 1347562A
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Images
Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/04—Hybrid capacitors
- H01G11/06—Hybrid capacitors with one of the electrodes allowing ions to be reversibly doped thereinto, e.g. lithium ion capacitors [LIC]
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/22—Electrodes
- H01G11/30—Electrodes characterised by their material
- H01G11/32—Carbon-based
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/22—Electrodes
- H01G11/30—Electrodes characterised by their material
- H01G11/46—Metal oxides
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/54—Electrolytes
- H01G11/58—Liquid electrolytes
- H01G11/62—Liquid electrolytes characterised by the solute, e.g. salts, anions or cations therein
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/425—Structural combination with electronic components, e.g. electronic circuits integrated to the outside of the casing
- H01M10/4264—Structural combination with electronic components, e.g. electronic circuits integrated to the outside of the casing with capacitors
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M14/00—Electrochemical current or voltage generators not provided for in groups H01M6/00 - H01M12/00; Manufacture thereof
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/621—Binders
- H01M4/622—Binders being polymers
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/13—Energy storage using capacitors
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y02T10/00—Road transport of goods or passengers
- Y02T10/60—Other road transportation technologies with climate change mitigation effect
- Y02T10/70—Energy storage systems for electromobility, e.g. batteries
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- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Power Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Microelectronics & Electronic Packaging (AREA)
- Materials Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Inorganic Chemistry (AREA)
- Secondary Cells (AREA)
- Battery Electrode And Active Subsutance (AREA)
- Electric Double-Layer Capacitors Or The Like (AREA)
Abstract
A rechargeable hybrid battery/supercapacitor electrical storage system capable of providing high energy and high power densities comprises an intercalation electrode (17) and a capacitor electrode (13) combined with a separator (15) and electrically-conductive current collector elements (11, 19) to form a unitary cell structure (10). An electrolyte solution of a dissociable salt absorbed into the porous structure of the separator (15) provides complementary ion species which respectively reversibly intercalate into the one electrode (17) and capacitively adsorb at the surface of the other electrode (13) upon the application of charging current. The high density stored electrical energy may be recovered at high power over extended periods upon demand of a utilizing device and may be rapidly restored to stable capacity through numerous charging cycles.
Description
Background of invention
The present invention relates to chargeable electric energy storage system many times, for electric application apparatus widely provides reliable power supply.The invention particularly relates to a kind of rechargeable storage system, it expresses the high-energy-density relevant with battery usually, and the high power density of ultra-capacitor representative and long service live.
In the present invention, this type systematic is a kind of energy storage device structure of multilayer, comprise many positive poles and negative pole element, each both positive and negative polarity element comprises dummy capacitor or double-deck ultra-capacitor material and the rechargeable insertion battery material that constitutes a monomer flexible structure, the size and shape of monomer flexible structure can determine as required, with the most compatible, and provide favourable high-energy-density and power density with application apparatus.
Modern Application needs removable power supply, and these application spread all over electric automobile from personal telecommunications apparatus, and quantity is index to be increased.These requirements that are applied on voltage for example or the power level are extensive, can provide high-energy-density rapidly in long-time always and can recharge light storage facility to the operating energy level very soon but all prefer to.So far, any in two kinds of existing type storage facilities, promptly such as rechargeable batteries such as lithium electronics insertion systems, the perhaps double-deck response type ultra-capacitor of induction type pseudocapacity ultra-capacitor or non-induction type, what satisfy these demands of removable energy widely.
Select battery or ultra-capacitor system usually by described application to high-energy-density or carry which more urgent deciding of high-power demand rapidly, wherein battery has high-energy-density, and ultra-capacitor can be carried high power rapidly.Battery in single application, meets high-energy and develops in some cases in the following manner with the trial of two kinds of demands of high power density two kinds of device kinds are arranged in, so that can charge to ultra-capacitor between the time period of high power requirements.Clearly, the shortcoming of this kind example is a preponderance.Other restriction of this example is reflected in the time demand of battery charge, and the diversity of battery and battery life cycle, and the physical property critical conditions of wherein inserting the battery charge operation can shorten battery life cycle usually.
System representation of the present invention goes out, and the device that meets removable electric energy application demand has tangible progress, and it is a light weight and enlarge and to combine the two necessary characteristic of battery and ultra-capacitor in the monomer integrating device of electric capacity.When system for example has can insert the comparative electrode that the battery pack compound forms by an activated carbon ultra-capacitor element and one time, be a kind of transition metal oxide spinel at described compound especially, its structure can be carried out the rapid diffusion of ion and be inserted under the few situation of back physical distortions, and this system can have the high energy storage ability of battery and the high speed energy delivery and the beat all life cycle of ultra-capacitor simultaneously.Induced cell inserts the unique combination of charging with capacitive surface and has another advantage, can realize such insertion system, they just can be reached because can for example adjust the held comparative electrode material rareness with quite big or small cation (for example, alkaline earth cation) size.
Hybrid system of the present invention can use previous rechargeable to insert most of composition of battery and ultra-capacitor device.These earlier device typically are described in for example United States Patent (USP) 5,418,091 and 5,115,378.As in these early stage systems, that inserts that electrode can comprise metal sulfide, oxide, phosphoric acid salt and fluoride, open architecture contains carbon graphite, hardening carbon and coke, and alloying element, such as aluminium, tin and silicon.Similarly, surface-active capacitor material, normally high surface area enclosed construction activated carbon powder, foaming body, fiber and textile, they can be used in the comparative electrode.The wherein active electrolyte element of hybrid system can be allocated by current material equally, and in the non-aqueous solution that can insert alkali metal and alkaline earth metal cation, use specific utility, this material is included in the material of fibre-bearing or polymer substrate with tangible fluid form usually, is the environment of a conducting of mobile maintenance of two kinds of electrolyte ion materials thus.The stacked polymer layer format description of secondary cell representative is in United States Patent (USP) 5,460,904, and relevant publication is applicable to structure of the present invention very much.
Summary of the invention
Invention hybrid battery/surpercapacitor structure comprises negative and positive electrode assembly in essence, and it has an insertion insulation ion penetration barrier assembly that comprises fluid electrolyte.It is good that these functional units are individual layers or iris-diaphragm stacked together, to form a kind of flexible single structure.Should comprise a kind of composition that inserts material by negative " battery " electrode assemblie layer, be good with a kind of spinel compound that is scattered in the polymeric matrices that for example gathers (vinylidene fluoride-copolymerization-hexafluoropropylene) copolymer.For interelectrode low resistance conduction of current is provided, but this battery layers heat lamination is in a conductive current collection assembly, such as a net metal paper tinsel.This just " ultra-capacitor " the same system of electrode assemblie layer made by a kind of activated carbon composition and a kind of electric current collection paper tinsel in copolymer matrix.
Between electrode assemblie, insert barrier assembly, its can comprise previous use height porosity, micropore shape or absorbable polymer thin layer or barrier film any one, be dispersed with a kind of a kind of cationic electrolyte salt solution, for example LiPF of inserting that comprise in these layers or the barrier film
6Stretch 1M solution in ethyl ester and the 1 umber dimethyl carbonate mixture at 2 umber carbonic acid.This kind electrolyte is guaranteed basic ionic conductivity and the mobility in this system configuration.Among the present invention, this mobility system flows into and the interest purpose that flows out individual electrode two kinds of ionic species of this electrolytic salt rapidly during according with this device charge and discharge.High fluidity can make this more greatly, before passivation and untapped anionic species produce more unrestricted moving, and to be adsorbed on positive electrode, it is in the electric capacity charging effect of participation system assembly herein.
Therefore, by from electrolyte the anion to this positive electrode surface move with for example this non-induction double deck type carry out electric capacity charging effect, improve the common cation that inserts (unique pattern that it typically is energy storage in the previous battery structure) in the charge period chien shih negative electrode and move.This kind induction is inserted battery charge and is produced high-energy-density rapidly with the effect that combines of non-inductive capacitor charging, and it can identical rapid mode recover, and looks application demand and produces high power density.By the property judged selection electrode material-be these indivedual insertions and electrode for capacitors modularization compounds that have required charging potential difference, can reach different voltage levels in this hybrid storage facility.
Summary of drawings
The present invention is described with reference to the drawings, wherein:
Fig. 1 is a schematic diagram, shows the cross section of a kind of stacked hybrid battery/surpercapacitor battery structure of the present invention;
Fig. 2 is a curve chart, shows the charging characteristic of typical each electrode of lithium ion insertion battery in the prior art;
Fig. 3 is a curve chart, shows the charging characteristic of typical double-deck each electrode of ultra-capacitor in the prior art;
Fig. 4 is a curve chart, shows the charging characteristic of each electrode in the hybrid battery/surpercapacitor system of the present invention;
Fig. 5 is a curve chart, shows the voltage level of individual electrode and compound hybrid system in one embodiment of the invention;
Fig. 6 is a curve chart, the charge volume of the hybrid battery/surpercapacitor system that shows one embodiment of the invention after through the charge/discharge cycle that prolongs; And
Fig. 7 shows the insertion voltage range of the multiple compound that can be used for making negative electrode in the hybrid system of the present invention.
Description of the invention
Fig. 1 shows the typical stacked hybrid battery/surpercapacitor structure 10 of the present invention (not to scale (NTS)) generally, it comprises a positive electrode assembly that comprises electric current collection paper tinsel 11, and the form of the preferably open aluminum mesh grid of described paper tinsel also has an end wing 12 that stretches out.The positive electrode assembly is laminated in electrode assemblie 13 under the effect of heat and pressure, and the latter comprises an activated carbon layer, such as a kind of carbon fiber textile or a kind of composition of the powder carbon in polymeric binder matrix.
The negative electrode assembly comprises electric current collection paper tinsel 19, and the form of the preferably open copper mesh grid of this paper tinsel also has an end wing 16.Equally, paper tinsel is laminated in one and inserts electrode assemblie 17, and the latter for example comprises a kind of polymeric matrices, and the insertion compound of be scattered here and there in the matrix a kind of (for example sub-micrometer range) in small, broken bits is such as preferable spinelle Li
4Ti
5O
12The structure of this preferred compounds advantageously has the insertion position of enough sizes, system's cation (Li for example
+) can hold rapidly and be dispersed in this crystal structure, and can not import the swelling stress that after long-time charge/discharge, may cause energy storage ability and useful life loss.Though famous spinelle in this regard clearly, a lot of other inserts material (such as famous publication and the hereinafter mentioned person of this specification) and can use in the active compound of native system negative electrode fully.
When the layer-built battery structure is finished, apply electrolyte solution a period of time of aforesaid kind, be enough to make electrolyte solution to absorb to the cavernous structure of barrier film 15 during this period of time, so that being provided in this system, moves in basic ion.Preferable electrolyte comprises the non-aqueous solution of dissociable salt, and these salts provide the insertion cation, such as alkali (Li for example
+), alkali earths (Mg for example
++), lanthanide series, Al
+++Or Zn
++Part.These electrolyte work to system equally, such as the anionic species of complementation, as PF
6 -, BF
4 -Or ClO
4 -
Shown in following embodiment, can more specifically make and use representative instantiation of the present invention.
Can successfully make the mode of rechargeable Li ion battery, such as the described mode of aforesaid patent specifications, preparation barrier film 15.Specifically, cast this barrier film with a kind of composition, described composition comprises a kind of 6 grams about 380 * 10
388: 12 of MW (sold by Atochem North America, be Kynar FLEX 2801) poly-(vinylidene fluoride-copolymerization-hexafluoropropylene) (VdF: HFP) copolymer and 10 grams can compatible organic plasticizer-dibatyl phithalates (DBP)-in about 40 solution that restrain in the acetone.The Powdered smog silica of other 4 grams is scattered in the solution in the mechanical type blender, casts said composition, and be dried to a kind of flexible diaphragm of about 0.075 millimeters thick.Said composition can comprise substituting plasticizer, such as rutgers, diethyl phthalate or phthalic acid three butoxy ethyl esters, and other inorganic filler additive, such as smoke-like aluminium oxide or silanization smoke-like silica.Said composition can be in order to strengthening the physical strength of barrier film, and in some composition, and electrolyte solution subsequently absorbs what can improve.
10 gram high surface area (1500 meters squared per gram) activated carbon powder are suspended in 88: 12 VdF of 20 grams: HFP copolymer (Atochem Kynar FLEX 2801) and the solution of 30 gram plasticizer (DBP) in about 160 gram acetone prepare a kind of positive electrode application composition thus.In a mechanicalness blender, stirred this mixture about 10 minutes, and really made it even, then casting and in air, making it dry 1 hour under the room temperature.The tough and tensile flexible ultra-capacitor electrode diaphragm 13 that forms is cut into about 50 millimeters * 80 millimeters required test size.The open aluminum mesh grid (for example accurate expansion paper tinsel of being sold by Delker Corporation of Microgrid) of about 50 micron thickness is cut the current collector element 11 (Fig. 1) into about 50 millimeters * 100 millimeters, and make it to contact with 13 in barrier film, so that about 20 millimeters end wing 12 that stretches out gatherer to be provided.Under the situation with the about 45N of every lineal cm contact pressure drum, this assemblage is passed through being heated between about 125 ℃ cylinder, in the cylinder contact position, the polymerization electrod composition of barrier film 13 is fully softening, penetrate the open net of net grid gatherer 11, and form the combination of firmly burying this gatherer, form a single positive electrode assembly.
Prepare a kind of negative pole with a kind of casting composition equally and insert electrode diaphragm, this casting composition comprises a kind of 10.5 gram pulverizing Li
4Ti
5O
12Restrain VdF with 1.2 gram Super-P conductive carbon powders at 2.8 of embodiment 1: the suspension in HFP copolymer and the 4.3 gram DBP solution in about 20 gram acetone.50 millimeters * 80 millimeters electrode diaphragms 17 are laminated in equally the electric current collection 19 of Microgrid expansion Copper Foil with an external part wing 16.Prepare this electrode assemblie and embodiment 2 to electrode the time, effective capacitor is provided carefully and comprises the reasonable balance of the indivedual quantity of insertion material of final electrode.It is benchmark that this kind equilibrium system is stored electric capacity with the predetermined power of individual electrode, and is mainly undertaken by the cast thickness of adjusting this barrier film.Therefore, in these examples, compared to 30 milliamperes/gram of electric capacity charging electrode, this insertion electrode provides higher ratio electric capacity, in other words about 150 milliamperes/gram, this negative electrode barrier film can be cast as a kind of thickness, makes this spinelle account for this positive electrode activated carbon compound quality about 20%.
Embodiment 4
Make the single hybrid battery/surpercapacitor cell apparatus that the present invention is specialized for finishing, arrange the indivedual positive electrodes and the negative electrode of preparation among the embodiment 2 and 3, wherein insert the barrier film of embodiment 1, with previous mode, use a kind of heated roller device-such as the stacked device of a kind of commercially available card form-in about 135 ℃ of following stacked these aggregations of temperature.Short circuit in this device is formed the end wing 12,16 of collector assembly by the lateral separation part of grid 11,19.
Final operation system in this manufacture method adds electrolyte solution and activates this hybrid battery pool device, reaching ionic conductivity, and provides the abundant container of an ionic species, to keep this charge/discharge cycle activity.In this respect, must be noted that native system not only uses for example Li of cationic substance
+As the charging of the activity during the reversible insertion in negative electrode place of previous storage battery transfer medium, it also is anionic species, for example PF
6 -, it carries out the reactive charge storage of double-deck ultra-capacitor in the positive electrode place.Therefore, can represent a kind of cationic source though one or more of previous battery system inserts electrode, in this hybrid system with the main source of electrolyte as two kinds of ionic species.Therefore provide abundant electrolyte support fully long-time and the recharge effect is very important.The electrolytical applied code of this kind system surpasses 2 to 5 times of stoichiometric.
Reach the abundant activation of these batteries easily with simple saturated this dividing plate of electrolyte solution, these batteries have and comprise the super porous membrane of prior formation, microfibrous barrier film or fiber mat, such as the structures such as barrier film of 0.5 millimeter Whatman borosilicate fiber filter plate.The battery structure of this example kind comprises electrode and plastification polymer composition, after in the copolymer compositions of this structure, extracting plasticizer, finish electrolytical interpolation and act as goodly via applying a kind of electrolyte solution, wherein the layer-built battery structure 10 of Fig. 1 is immersed in the solvent (its influence for copolymer based material is quite little) that a kind of plasticizer uses and carry out this extraction.As for above-mentioned VdF:HFP copolymer, this kind solvent can be diethyl ether or dimethyl ether, methyl alcohol, hexane etc.Slowly evaporate this extraction solution by the barrier film appropriateness, the micropore shape structure that forms in whole barrier film 15 provides abundant position to layer-built battery 10, before holds any non-aqueous electrolytic solution commonly used in polymerization cell and the ultra-capacitor to keep.
Noteworthyly be, can be in this electrolyte solution with an organic solvent, such as propene carbonate, diethoxyethane, diethyl carbonate, dimethoxy-ethane, sulfolane and dipropyl carbonate and composition thereof.In addition, during allotment activation electrolytic matter solution, suitable lithium salts comprises LiClO
4, LiN (CF
3SO
2)
2, LiBF
4, LiCF
3SO
3And LiSbF
6, its can be used between about 0.5 and 2M between solution concentration.Useful especially is beat all LiPF
6Ethylene carbonate/dimethyl carbonate composition and and U.S.5,192,629 described LiBF
4Mixture.
Embodiment 5
When using this kind preparation of electrolyte, stacked polymerization cell structure 10 is dipped in a kind of diethyl ether body,, extracts the DBP component and the barrier film composition of this electrode in about 10 minutes of gentle agitation wherein.Remove and after drying at room temperature from this extraction tank, under no moisture atmosphere, immerse LiPF
6In ethylene carbonate (EC): dimethyl carbonate (DMC) is about 10 minutes of 2: 1 1M electrolyte solutions in the mixture activating this battery, during this electrolyte solution suck in this micropore shape stepped construction, roughly replace original DBP plasticizer.Then, gently wipe away to remove surperficial electrolyte with absorbing material, outside this end wing 12,16 that stretches out, activation battery/ultra-capacitor battery 10 is sealed in a kind of polyolefin packing (not showing), to keep no moisture environment.
Embodiment 6
During making, sample with regard to a kind of aforementioned hybrid battery of test objective correction/ultra-capacitor cell apparatus, it is that a silver-colored line electrode 14 is inserted in the barrier films 15, so that common reference to be provided, measures voltage characteristic during this device charge/discharge cycle with reference to this data.In order to compare, when carrying out the charge/discharge cycle test, the Li/CLi ion of revising indivedual Prior Arts equally inserts battery and the double-deck ultra-capacitor battery of C/C.This Ag dummy electrode provides in fact approaching zero data with relative voltage (with respect to-0.05 volt approximately of standard hydrogen electrode (SHE)), with the battery-operated chart of this data plotting, and during the charge and discharge ringing, the differentiation that the voltage of individual electrode changes.
In this mode, operation is in conjunction with stacked PVdF:HFP barrier film and LiPF
6: during the electrolytical previous battery of EC:DMC, can follow the trail of for example Li as shown in Figure 2
+Ion each just with negative Li
xMn
2O
4With going insertion and inserting the voltage level on the graphite electrode, wherein the voltage level 24,26 of these electrodes arrives+1.0 volts and-3.1 volts approximately, produces about 4.01 volts complete charged battery voltage.On the contrary, as shown in Figure 2, during this battery discharge, Li
+The conceited graphite electrode of ion goes to insert, and is inserted in the positive spinel electrode, and individual electrode voltage is got back to master data.
Embodiment 7
In the same manner, change characteristic at the voltage during the double-deck ultra-capacitor drafting of the stacked polymer substrate of the Prior Art that comprises the active carbon electrode barrier film charge/discharge cycle.This structure is similar with Fig. 1 substantially, and it is the electrolyte that uses PVdF:HFP copolymer and embodiment 6.As shown in Figure 3, each cycle period, be the representative of electric capacity charging from 22 to+1.25 volts of indivedual charging electrode voltage 34,36 symmetries and rule variations of basic document, and reflect the analogous composition of these electrodes with-1.25 volts.
Embodiment 8
Carry out the hybrid battery/surpercapacitor instantiation test cell of embodiment 6 with previous mode, as shown in Figure 4, draw the electrode voltage characteristics with the false standard basic document 42 of Ag.Plant assessment thus and find, can find out that indivedual positive excess capacitor bank thing electrodes and negative battery insert composition electrodes and possess its tangible charging characteristic 44,46, its basic document between+1.25 volts and-1.25 volts and the level of charging fully.These representative charging cycle profiles are determined the function of hybrid battery, wherein in when charging, and this electrolytical Li
+Ion inserts the Li of negative electrode
4Ti
5O
12In the spinelle, provide battery high-energy-density electric charge 46, and PF
6 -Electrolyte ion is adsorbed in positive active carbon electrode, produces high power density supercapacitors electric charge 44.As shown in Figure 5, the mixed function of these electrodes provides along the indivedual charging voltages of track 54,56 accumulation, and it produces a linear-charging voltage range 58, provides relevant with data 52, between about 1.5 volts with 2.75 volts high-energy and power density.
On all tracks 62 of Fig. 6, after constant 1.12 milliamperes of long-time operations, the unusual stable electric capacity of this hybrid battery/surpercapacitor as can be seen.This advantageous feature reflects with Li
4Ti
5O
12The significant of spinelle negative electrode is strengthened the ultra-capacitor height of devices stability of this instantiation, and wherein this negative electrode character can be inserted effect, and can not make this spinel structure produce degraded physics swelling stress.
Can use in hybrid battery of the present invention and have different successful degree other insert material and comprise sulfide, such as TiS
2, FeS
2With ZrS
2Oxide is such as MnO
2, LiMn
2O
4, MoO
3, WO
3, TiO
2, Co
3O
4, Fe
2O
3With Cr
3O
8Phosphoric acid salt is such as LiFePO
4With LiMnPO
4Fluoride is such as FeF
2With FeF
3Carbonaceous material is such as graphite, coke and hardening carbon; And alloying metal and compound, such as Al, Sn, SnO
2With Si.In order to obtain the important operation voltage range with this hybrid system, it is good with having the material that inserts voltage range that selectivity is inserted compound, and these scopes are starkly lower than the electric capacity charging scope through selectivity ultra-capacitor electrode material (for example activated carbon).The insertion voltage range that many suitable negative electrode materials and SHE data are compared is shown in Fig. 7.Also find to use comparatively simpler method evaluate electrode and the electrolyte and the system operation of mechanicalness Swagelock test portion battery unit satisfactorily.Testing data can be considered that the data of layer-built battery is suitable more completely with the described development of previous examples.
Expection is familiar with this skill person via utilizing original character can obtain other variation of the hybrid battery/surpercapacitor system that aforementioned narration discloses, and these variations comprise in the scope of the invention that appended claims states.
Claims (20)
1. rechargeable electric energy storage system, its contact ground comprise a positive electrode assembly, negative electrode assembly and insertion and contain a kind of barrier assembly of fluid electrolyte therebetween, and described electrolyte comprises the ionic species of a pair of dissociable salt,
It is characterized in that,
A) one of described electrode assemblie comprises and a kind ofly can insert first kind of ionic species, changes the material of using to adapt to first polarity electricity, and
B) another of described electrode assemblie comprises and a kind ofly can adsorb second kind of ionic species, changes the material of using to adapt to the simultaneous electricity of relative polarity.
2. storage system as claimed in claim 1 is characterized in that, described first ionic species is selected from the group that comprises bases, alkali earths, lanthanum class, Al and Zn.
3. storage system as claimed in claim 1 is characterized in that, described second ionic species is selected from and comprises PF
6, ClO
4, BF
4, CF
3SO
3And SbF
6Group.
4. storage system as claimed in claim 1 is characterized in that, the material of a described electrode assemblie is selected from and comprises transition metal oxide, sulfide, phosphoric acid salt and fluoride, and the group of alkali metal and alkaline-earth metal-alloying metal and compound.
5. storage system as claimed in claim 1 is characterized in that, the material of a described electrode assemblie is selected from and comprises that open architecture contains the group of carbon graphite, hardening carbon and coke.
6. storage system as claimed in claim 1 is characterized in that, the material of described another electrode assemblie is selected from the group that comprises dummy capacitor and electrode of electric double layer capacitor material.
7. storage system as claimed in claim 4 is characterized in that the material of a described electrode assemblie is selected from the group that comprises the transition metal oxide spinel compound.
8. storage system as claimed in claim 7 is characterized in that the material of a described electrode assemblie is Li
4Ti
5O
12
9. storage system as claimed in claim 6 is characterized in that, the material of described another electrode assemblie is selected from the group that comprises high surface area activated carbon powder, foaming body, fiber and textile material.
10. storage system as claimed in claim 1, it is characterized in that, described electrolyte comprises 0.5M to the 2.0M solution of at least a described dissociable salt in organic solvent, and described solvent is selected from the group that comprises ethylene carbonate, dimethyl carbonate, propene carbonate, diethoxyethane, diethyl carbonate, dimethoxy-ethane, sulfolane and dipropyl carbonate and composition thereof.
11. storage system as claimed in claim 10 is characterized in that, described at least a dissociable salt is selected from and comprises LiPF
6, LiClO
4, LiN (CF
3SO
2)
2, LiBF
4, LiCF
3SO
3With LiSbF
6Group.
12. rechargeable hybrid battery/surpercapacitor system, this system comprises that a positive electrode assembly, negative electrode assembly and insertion are and comprise a kind of barrier assembly of fluid electrolyte therebetween, described electrolyte comprises the ionic species of a pair of dissociable salt
It is characterized in that,
A) one of described electrode assemblie comprises layer of material, and this layer material can insert first kind of ionic species, changes application to adapt to first polarity electricity, and
B) another of described electrode assemblie comprises layer of material, and this material can adsorb second kind of ionic species, changes application to adapt to the simultaneous electricity of relative polarity,
C) described barrier assembly comprises a micropore shape layer, wherein is dispersed with the non-aqueous solution of described dissociable salt, and
D) described each assembly is bonding with one or more adjacent assemblies on interface separately at it, forms a single stepped construction.
13. hybrid system as claimed in claim 12 is characterized in that, each described electrode assemblie is bonding with electrically conductive, electrically flow collector element separately.
14. hybrid system as claimed in claim 12 is characterized in that,
A) each described electrode assemblie layer includes a kind of polymeric matrices, and the ion that wherein is dispersed with separately inserts and ion adsorbing material,
B) described barrier assembly layer comprises a kind of polymerization barrier film, wherein is dispersed with a lot of holes and space, and
C) to act on its polymeric surface place by heat bonding bonding for described all assemblies.
15. hybrid system as claimed in claim 12 is characterized in that, the material of a described electrode assemblie is selected from and comprises transition metal oxide, sulfide, phosphoric acid salt and fluoride, and the group of alkali metal and alkaline-earth metal-alloying metal and compound.
16. hybrid system as claimed in claim 12 is characterized in that, the material of a described electrode assemblie is selected from the group that contains carbon graphite, hardening carbon and coke that comprises open architecture.
17. hybrid system as claimed in claim 12 is characterized in that, the material of described another electrode assemblie is selected from the group that comprises dummy capacitor and electrode of electric double layer capacitor material and high surface area activated carbon powder and fiber.
18. hybrid system as claimed in claim 12, it is characterized in that, described electrolyte comprises 0.5M to the 2.0M solution of at least a described dissociable salt in organic solvent, described solvent be selected from comprise ethylene carbonate, dimethyl carbonate, propene carbonate, diethoxyethane, diethyl carbonate, dimethoxy-ethane, sulfolane, with the group of dipropyl carbonate and composition thereof.
19. hybrid system as claimed in claim 18 is characterized in that, described at least a dissociable salt is selected from and comprises LiPF
6, LiClO
4, LiN (CF
3SO
2)
2, LiBF
4, LiCF
3SO
3With LiSbF
6Group.
20. hybrid system as claimed in claim 12 is characterized in that,
A) a described electrode assemblie layer comprises Li
4Ti
5O
12,
B) described another electrode assemblie layer comprises a kind of high surface area activated carbon, and
C) described electrolyte comprises LiPF
6In ethylene carbonate: dimethyl carbonate is 2: the 1 1M solution in the mixture.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| US09/295,537 US6252762B1 (en) | 1999-04-21 | 1999-04-21 | Rechargeable hybrid battery/supercapacitor system |
| US09/295,537 | 1999-04-21 |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN1347562A true CN1347562A (en) | 2002-05-01 |
Family
ID=23138126
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN00806515A Pending CN1347562A (en) | 1999-04-21 | 2000-04-19 | Rechargeable hybrid battery/surpercapacitor system |
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| Country | Link |
|---|---|
| US (1) | US6252762B1 (en) |
| EP (1) | EP1185991B1 (en) |
| JP (1) | JP4465492B2 (en) |
| KR (1) | KR20010112443A (en) |
| CN (1) | CN1347562A (en) |
| AU (1) | AU768608B2 (en) |
| CA (1) | CA2370217C (en) |
| IL (1) | IL145939A0 (en) |
| MY (1) | MY122514A (en) |
| TW (1) | TW463409B (en) |
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| MY122514A (en) | 2006-04-29 |
| EP1185991A1 (en) | 2002-03-13 |
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| WO2000063929A1 (en) | 2000-10-26 |
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| EP1185991B1 (en) | 2012-10-31 |
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| EP1185991A4 (en) | 2007-10-17 |
| JP2002542582A (en) | 2002-12-10 |
| JP4465492B2 (en) | 2010-05-19 |
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